Tantalum (Ta) is a refractory metal having a high melting point, a low electrical resistivity, and which is generally inert at temperatures below about 150° C. Alpha-tantalum (α-Ta) is the bulk equilibrium or stable-phase of tantalum. α-Ta has numerous applications in magnetic thin films devices including magnetic disk hard drives, and as diffusion barriers in integrated circuits fabrication where copper interconnect technology is used. Because of its numerous uses, there remains a need for methods of forming α-Ta.